Creation of clean interfaces without contamination of adventitious carbon and robust single active sites are highly desirable for delivery and utilization of electrons in sunlight-driven hydrogen production but still remains challenging in part owing to the lack of understanding in junction nature. Herein, we tackle this challenge by targeted removing of interfacial adventitious carbon between photoharvester CdS and novel single-cobalt co-catalyst (Co-NC). It's found that surface-trapped electrons can readily migrate to the closely attached Co-NC across the cleared interface between CdS and Co-NC. The small-resistance interfacial carrier path and the robust single-cobalt sites work in a cooperative way and hence achieve a superior visible-light driven H₂ generation activity with a rate of 4.34 mmol/h, an apparent quantum yield (AQY) of 63.9% at 400 nm and a ultrahigh turnover frequency (TOF) of up to 16714.7 h⁻¹. Our finding will motivate future work in creating clean interfaces and unique single active sites for high performance photocatalysis.

对于在阳光驱动的氢生产中电子的传递和利用，非常需要创建无污染的碳和坚固的单个活性位点的清洁界面，但是由于缺乏对结点性质的了解，仍然存在挑战。本文中，我们通过有针对性地去除光敏收割剂CdS和新型单钴助催化剂（Co-NC）之间的界面不定碳来应对这一挑战。已经发现，表面俘获的电子可以很容易地穿过CdS和Co-NC之间清除的界面迁移到紧密相连的Co-NC。小电阻的界面载流子路径和坚固的单钴位点以协同方式工作，因此可实现出色的可见光驱动的H ₂产生活性，速率为4.34 mmol / h，400 nm时的表观量子产率（AQY）为63.9％，超高周转频率（TOF）高达16714.7 h ^-1。我们的发现将激励未来为高性能光催化创建干净的界面和独特的单个活性位点的工作。